CN102690681B - Catalytic cracking method for producing propylene - Google Patents
Catalytic cracking method for producing propylene Download PDFInfo
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- CN102690681B CN102690681B CN201110072782.6A CN201110072782A CN102690681B CN 102690681 B CN102690681 B CN 102690681B CN 201110072782 A CN201110072782 A CN 201110072782A CN 102690681 B CN102690681 B CN 102690681B
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
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- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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- Y02P20/584—Recycling of catalysts
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Abstract
The invention discloses a catalytic cracking method for producing propylene. The catalytic cracking method comprises that one or more heavy raw materials and a catalyst containing shape-selective zeolite having an average aperture size less than 0.7nm undergo a cracking reaction in a first riser reactor; and one or more light hydrocarbons and a catalyst having a temperature of 550 to 690 DEG C and containing shape-selective zeolite having an average aperture size less than 0.7nm undergo a cracking reaction in a second riser reactor and a fluidized bed reactor. The catalytic cracking method can be used for heavy oil catalytic cracking, and has a high heavy oil conversion rate, a high propylene yield and low dry gas and coke yields.
Description
Technical field
The present invention relates to a kind of catalyst cracking method.
Background technology
Heavy oil catalytic pyrolysis is the important method of preparing the small-numerator olefins such as ethene, propylene and butylene.The method of the heavy oil fluid catalytic cracking production low-carbon alkene of industrial use comprises the catalytic pyrolysis technology (DCC of maximum production of propylene, USP4980053 and USP5670037) and maximum produce the catalytic pyrolysis technology (CPP of ethene, USP6210562), these two kinds of methods adopt single riser reactor or the combined fluidized bed structure of reactor of single riser reactor to coordinate special-purpose catalyst to react under higher temperature conditions.Although above-mentioned two kinds of existing patented technologies can be produced the low-carbon alkenes such as propylene, ethene, but its dry gas and coke yield are also relatively high, and its productivity of propylene is difficult to further raising, the heavy oil conversion degree of depth that is difficult to not only to keep higher and higher high-value product yield are simultaneously but also do not increase the productive rate of dry gas, coke.
CN1140608C discloses a kind of regenerated catalyst method of cooling, to partial regeneration agent, carry out cooling, the cooled regenerator of a part mixes at the pre lift zone of riser tube with uncooled high temperature regeneration agent, the mixed catalyst of relatively lower temp again with hydrocarbon ils contact reacts, simultaneously the cooled regenerator of another part returns to revivifier regulation and control regeneration temperature.The method does not relate to raising productivity of propylene.
CN1081222C discloses a kind of catalysis conversion method that reduces olefin(e) centent in liquefied gas and gasoline.The bottom that the method proposition enters the hydrocarbon oil crude material after preheating riser tube in the compound reactor of single riser tube or single riser tube and fluidized-bed formation contacts with catalyzer, reacted oil gas logistics goes upward to riser tube middle part or riser tube top contacts, reacts with the catalyzer after cooling, and reactant flow is carried out follow-up separating obtained product through settling vessel bleeder.Reacted catalyzer is divided into two portions after high temperature coke burning regeneration, and a part enters riser tube bottom, and a part enters riser tube middle part or riser tube top through overcooling is laggard, but the method is unfavorable for producing propylene and other small-numerator olefin.
CN1428402A discloses a kind of catalytic cracking combination process, comprise that the regenerator of 10～80 heavy % is entered to circular fluidized-bed reactor after cooling to be contacted, react with gasoline stocks, reacted catalyzer enters the stripping zone of circular fluidized-bed reactor and carries out stripping; The heavy % of catalyzer after stripping 40～90 return to reaction zone and recycle, rest part after delivering to and mixing with uncooled high temperature regeneration agent before the pre lift zone of heavy oil riser tube again with heavy hydrocarbon oil contact reacts.The method has realized raising heavy oil conversion performance, reduces olefin(e) centent in gasoline, but does not propose method and the approach how propylene enhancing reduces dry gas simultaneously, and its productivity of propylene is lower.
CN1177020C discloses a kind of inferior gasoline upgrading method and device thereof.The method is transported to stripping stage after proposing that regenerator is cooled to 300 ℃～500 ℃ mixes with spent agent for reacting with inferior patrol counter current contact, olefin(e) centent and sulphur content, raising gasoline RON in reduction gasoline, but do not relate to propylene enhancing.
Summary of the invention
The technical problem to be solved in the present invention is for the low deficiency of existing catalytic cracking for producing propylene using method productivity of propylene, and a kind of catalyst cracking method that can improve the production propylene of productivity of propylene is provided.
The invention provides a kind of catalyst cracking method of producing propylene, comprising:
(1) by heavy feed stock and first strand of catalytic cracking catalyst in the first riser reactor contact reacts, by the tripping device of the first riser reactor end, carbon deposited catalyst after oil gas and reaction is separated, it is separated that oil gas is introduced product separation system; What first strand of described catalytic cracking catalyst was less than 0.7nm containing mean pore size selects shape zeolite;
(2) by light hydrocarbon and temperature, be that second strand of catalytic cracking catalyst of 550 ℃～690 ℃ introduced the second riser reactor contact reacts, reacted oil gas and catalyzer introduced to the fluidized-bed reactor of connecting with the second riser reactor and react; It is separated that the reacted oil gas of fluidized-bed reactor is introduced product separation system, and carbon deposited catalyst recycles after stripping, regeneration.Described lightweight gently comprises gasoline and/or the C4 hydrocarbon that described product separation system obtains; What second strand of described catalytic cracking catalyst was less than 0.7nm containing mean pore size selects shape zeolite.
The present invention also provides a kind of device of the method for above-mentioned For Producing Propylene in Fcc, and this device comprises the first riser reactor, the second riser reactor, fluidized-bed reactor, stripper, settling vessel, product separation system, revivifier and catalyzer heat collector; Wherein the second riser reactor is connected with fluidized-bed reactor, fluidized-bed reactor is communicated with stripper and settling vessel, the first riser reactor is connected with settling vessel, and catalyzer heat collector is communicated with the second riser reactor and revivifier respectively by catalyst transport.
The catalyst cracking method of production propylene provided by the invention, the combined reactor based on double lifting leg and fluidized-bed formation, by the optimization of process program, be equipped with suitable catalyzer, different feeds is carried out to selective conversion, can improve productivity of propylene, there is lower dry gas and coke yield.
Accompanying drawing explanation
Fig. 1 is the schematic diagram of catalytic cracking unit provided by the invention.Wherein 1,2 is riser reactor, and 3 is stripper, and 4 is fluidized-bed reactor, and 5 is that settling vessel, 6 is that product separation system (or claiming product separation device), 7 is revivifier.8 is reclaimable catalyst inclined tube (control catalyst flow wherein by guiding valve aperture, do not mark in figure), and 9 and 10 is regenerated catalyst inclined tube (control catalyst flow wherein by guiding valve aperture, do not mark in figure).40 is external catalyst cooler for regenerator, and 41 is regenerator inclined tube after cooling process.As shown in Figure 1, riser reactor 2 is realized and being arranged in juxtaposition with riser reactor 1 by settling vessel 5 with coaxial series connection of fluidized-bed reactor 4, simultaneously with 3 coaxial being connected of height of stripper.
Embodiment
According to the catalyst cracking method of production propylene provided by the invention, heavy feed stock and first strand of catalytic cracking catalyst are in the first riser reactor contact reacts, tripping device by riser tube end is separated with reacted carbon deposited catalyst by oil gas, and it is separated that oil gas is introduced follow-up product separation system; First strand of catalytic cracking catalyst of carbon deposit introduced stripper or the follow-up described fluidized-bed reactor of the present invention.Part or all of the gasoline simultaneously product separation system separation being obtained and/or C4 hydrocarbon and second strand of catalytic cracking catalyst are in the second riser reactor contact reacts.The tripping device of described riser tube end is for separated with carbon deposited catalyst by reacted oil gas, this is conducive to reduce dry gas yied, suppresses especially propylene transforming again after generating of low-carbon alkene, described tripping device is preferably fast separating device, can adopt existing fast separating device, preferred fast packing is set to slightly revolves a minute separator.The first riser reactor operation condition comprises: temperature of reaction (riser reactor temperature out) is 480～600 ℃, preferably 500～560 ℃, agent-oil ratio is 5～20, be preferably 7～15, the reaction times is 0.50～10 second, is preferably 2～4 seconds, atomized water steam accounts for 2～50 % by weight of heavy feed stock inlet amount, be preferably 5～10 % by weight, reaction pressure is 0.15～0.3MPa (absolute pressure), is preferably 0.2～0.25MPa.
In catalyst cracking method provided by the invention, described heavy feed stock is heavy hydrocarbon or the various animals and plants oils raw materials that are rich in hydrocarbon polymer, and described heavy hydrocarbon is selected from one or more the mixture in petroleum hydrocarbon, mineral oil and synthetic oil.Petroleum hydrocarbon is conventionally known to one of skill in the art, for example, can be the hydrocarbon ils that decompressed wax oil, long residuum, decompressed wax oil blending part vacuum residuum or other secondary processing obtain.The hydrocarbon ils that described secondary processing obtains is as one or more in raffinating oil of wax tailings, deasphalted oil, furfural treatment.Mineral oil is selected from one or more the mixture in liquefied coal coil, tar sand oil and shale oil.Synthetic oil is that coal, Sweet natural gas or pitch are through the synthetic distillate obtaining of F-T.The described various animals and plants oils raw materials that are rich in hydrocarbon polymer are animal grease and Vegetable oil lipoprotein for example.
The catalyst cracking method of production propylene provided by the invention, by temperature, be that 570 ℃～690 ℃ second strand of catalytic cracking catalysts and light hydrocarbon are introduced after the second riser reactor contact reacts, reacted oil gas is introduced to the fluidized-bed reactor contact reacts of connecting with the second riser reactor with catalyzer; It is separated that the reacted oil gas of fluidized-bed reactor is introduced subsequent product separation system, and carbon deposited catalyst recycles after stripping, regeneration.More preferably 570～680 ℃ of the temperature of second strand of catalytic cracking catalyst of described introducing the second riser reactor.Second strand of catalytic cracking catalyst introducing the second riser reactor is generally the regenerator from revivifier; needs due to regeneration; the temperature of regenerator conventionally can be higher than 700 ℃; for this reason; regenerator first carries out heat-obtaining cooling process; being cooled to temperature is 550 ℃～690 ℃, is preferably 570～680 ℃.
The catalyst cracking method of the production propylene of confession of the present invention, second strand of catalytic cracking catalyst with through the light hydrocarbon of atomization, introduce the second riser reactor bottom contact reacts, the mixing temperature of contact is preferably 530 ℃～680 ℃, more preferably 550 ℃～660 ℃ of described mixing temperatures, more more preferably 630 ℃～650 ℃.The agent-oil ratio (introducing second strand of catalytic cracking catalyst and the weight ratio of introducing the light hydrocarbon of the second riser reactor of the second riser reactor) of light hydrocarbon being introduced to the second riser reactor reaction is 5～40.
Described light hydrocarbon is gasoline fraction and/or C4 hydrocarbon.When comprising gasoline fraction, the operation condition of gasoline fraction in the second riser reactor: it is 10～30 that gasoline fraction operates agent-oil ratio (introducing the catalyzer of the second riser reactor and the weight ratio of gasoline fraction) in the second riser reactor, is preferably 15～25; Reaction times is 0.10～1.5 second, preferably 0.30～0.8 second; Gasoline atomizing water vapor accounts for 5～30 % by weight of gasoline feeding amount, preferably 10～20 % by weight.When comprising C4 hydrocarbon, the operation condition of C4 hydrocarbon: it is 12～40 that C4 hydrocarbon operates agent-oil ratio (introduce the catalyzer of the second riser reactor and the weight ratio of C4 hydrocarbon) in the second riser reactor, preferably 17～30; C4 hydrocarbon reaction times in the second riser reactor is 0.50～2.0 second, preferably 0.8～1.5 second; C4 hydrocarbon atomized water steam accounts for 10～40 % by weight of C4 hydrocarbon inlet amount, preferably 15～25 % by weight.Introducing the light hydrocarbon of the second riser reactor and the weight ratio of heavy feed stock is 0.05～0.5: 1.
In catalyst cracking method provided by the invention, the operation condition of fluidized-bed reactor comprises: reaction pressure is 0.15～0.3MPa (absolute pressure), is preferably 0.2～0.25MPa; Fluidized-bed reaction temperature is 500～580 ℃ (bed temperatures), is preferably 510～560 ℃; The weight hourly space velocity of fluidized-bed reaction (combined feed total feed of fluid bedreactors hydrocarbon) is 1～35 hour
-1, be preferably 3～30 hours
-1.
In catalyst cracking method provided by the invention, the light hydrocarbon of introducing the second riser reactor is gasoline fraction and/or C4 hydrocarbon, is preferably the gasoline fraction and/or the C4 hydro carbons that are rich in alkene.Described gasoline fraction is selected from the gasoline of this device self-produced (described product separation system obtains) and/or the gasoline fraction that other device is produced.The mixture of one or more in the gasoline fraction that the optional catalytic cracking raw gasline of gasoline fraction, catalytic cracking stable gasoline, coker gasoline, viscosity breaking gasoline and other oil refining that other device is produced or chemical process are produced, preferentially selecting is that this installs self-produced gasoline fraction.The olefin(e) centent of described highly olefinic gasoline cut is 20～95 % by weight, and preferred 35～90 % by weight, more than being preferably in 50 % by weight.Described gasoline stocks can be the gasoline fraction of full range, final boiling point be no more than 204 ℃ for example boiling range be the gasoline fraction of 30～204 ℃, also can be narrow fraction wherein, the gasoline fraction of boiling range between 30～85 ℃ for example, preferably boiling range is the gasoline fraction of 30～85 ℃.The gasoline fraction of introducing the second riser reactor is 0.05～0.20: 1 with the weight ratio of introducing the heavy feed stock of the first riser reactor, be preferably 0.08～0.15: 1, the preferred highly olefinic gasoline cut of described gasoline fraction, more preferably this installs self-produced highly olefinic gasoline cut.Described C4 hydro carbons refers to take the low-molecular-weight hydrocarbon existing with gas form under normal temperature that C 4 fraction is main component, normal pressure, comprises alkane, alkene and alkynes that in molecule, carbonatoms is 4.It can be the self-produced gaseous hydrocarbon products that is rich in C 4 fraction of this device, can be also the hydrocarbon gas that is rich in C 4 fraction that other device or process are produced, and wherein preferably this installs self-produced C 4 fraction.Described C4 hydrocarbon is preferably the C 4 fraction that is rich in alkene, and wherein the content of C4 alkene is greater than 50 heavy %, is preferably greater than 60 heavy %, preferably more than 70 % by weight.Preferred described light hydrocarbon comprises gasoline fraction, containing or containing C4 hydrocarbon, the weight ratio of C4 hydrocarbon and gasoline fraction is 0～2: 1, preferably 0～1.2: 1, most preferably 0～0.8: 1.
In the catalyst cracking method of production propylene provided by the invention, light hydrocarbon is introduced to the second riser reactor, after the second riser reactor reaction, introduce fluidized-bed reactor and continue reaction.Preferably, the cracking masout also product separation system of the present invention being obtained is introduced and in the second riser reactor, is reacted and/or introduce fluidized-bed reactor and react; When cracking masout is introduced the second riser reactor, the introducing location optimization of described cracking masout at 1/2nd places of riser tube length to the i.e. postmedian of the second riser reactor of the part of leg outlet, preferably, described cracking masout is introduced in fluidized-bed reactor and is reacted, and more preferably introduces the bottom of described fluidized-bed reactor.Described cracking masout is the cracking masout that product separation system of the present invention obtains, and the crackate that enters product separation system is isolated remaining most of product liquid after gas, gasoline and diesel oil.The normal pressure boiling range of described cracking masout is between 300～550 ℃, and preferably its normal pressure boiling range is 350～530 ℃.The cracking masout of introducing the second riser reactor and fluidized-bed reactor is 0.05～0.35: 1 with the weight ratio of introducing the heavy feed stock of the first riser reactor, preferably 0.05～0.25: 1.While preferably injecting described cracking masout, the coke content on catalyst reactor is no more than 0.5 % by weight, is preferably 0.1～0.3 % by weight.Cracking masout is introduced in riser reactor middle and lower reaches or fluidized-bed reactor, realize on the one hand the heavy oil conversion degree of depth that heavy oil twice transformation improves whole device, utilize cracking masout cut propylene enhancing, the Quench of gasoline fraction and/or C4 hydrocarbon reaction is stopped simultaneously, suppress low-carbon alkene, especially propylene generates conversion reaction more afterwards, improves simultaneously and generates Propylene Selectivity.The operation condition of the second riser tube and cracking masout cut in fluidized-bed tandem reactor: the agent-oil ratio that catalyzer contacts with cracking masout (weight ratio) is 1～50, preferably 5～40; Cracking masout atomized water steam accounts for 5～20 % by weight of described cracking masout inlet amount, preferably 10～15 % by weight.
In catalyst cracking method provided by the invention, the tripping device of the first riser reactor end is separated with carbon deposited catalyst by reaction oil gas, and oil gas enters follow-up product separation system after further isolating the catalyzer wherein carrying.The reacted oil gas of fluidized-bed reactor, after settling vessel is isolated the catalyzer carrying wherein, enters follow-up product separation system.In product separation system, oil gas is isolated to cracked gas, pyrolysis gasoline, cracking light oil and cracking masout.Described product separation system can adopt prior art, and the present invention does not have particular requirement.
In catalyst cracking method provided by the invention, the carbon deposited catalyst that the tripping device separation of the first riser reactor end obtains can directly be introduced stripping system and carry out stripping, also can first introduce fluidized-bed reactor, after catalyst mix in fluidized-bed reactor, enter again stripping system and carry out stripping, preferably first introduce and enter again stripper after fluidized-bed reactor and carry out stripping.The cracking catalyst of leaving fluidized-bed reactor enters stripper and carries out stripping, two strands of catalyzer stripping in same stripper, catalyzer after stripping is introduced revivifier regeneration, and the first riser reactor introduced by the catalyzer after regeneration and the second riser reactor recycles.
In catalyst cracking method provided by the invention, the oil gas that water stripping steam and stripping go out, the bottom of preferably introducing fluidized-bed reactor, through after fluidized-bed, discharge reactor, can reduce oil gas dividing potential drop, shorten oil gas in the settling section residence time, propylene enhancing reduces dry gas, coke yield simultaneously.
In catalyst cracking method provided by the invention, described riser reactor be selected from equal diameter riser tube, etc. linear speed riser tube and straighten a kind of or wherein combination of two kinds in the riser tube of footpath, wherein the first riser reactor and the second riser reactor can adopt identical pattern also can adopt different patterns.That described fluidized-bed reactor is selected from is fixed fluidized bed, one or more the combination in dispersion fluidized bed, bubbling bed, turbulent bed, fast bed, conveying bed and dense bed reactor.
In catalyst cracking method provided by the invention, the cat-cracker using at least comprises reactor part, revivifier part and product separation system, preferred reactor adopts double lifting leg and fluidized-bed to form combined reactor configuration, one of them riser tube is connected preferably coaxial series connection afterwards with fluidized-bed reactor and another riser tube is arranged in juxtaposition mutually, and described riser tube and the coaxial cascaded structure of fluidized-bed further with the preferred coaxial coupled arrangement of stripper coupled arrangement.
In described riser tube and the coaxial series combination of fluidized-bed reactor, leg outlet preferably includes low tension outlet sparger, and its pressure drop is less than 10KPa.Described low tension outlet sparger is arch sparger for example.
In catalyst cracking method provided by the invention, what described catalyzer contained that mean pore size is less than 0.7 nanometer selects shape zeolite, and what first strand of catalytic cracking catalyst and second strand of catalytic cracking catalyst all contained that mean pore size is less than 0.7 nanometer selects shape zeolite.The shape zeolite of selecting that described mean pore size is less than 0.7 nanometer is selected from ZSM series zeolite, ferrierite, chabazite, dachiardite, erionite, A zeolite, epistilbite, lomontite, and one or more the mixture among the above-mentioned zeolite obtaining after physics and/or chemical process are processed.ZSM series zeolite is selected from one or more the mixture in the zeolite of ZSM-5, ZSM-8, ZSM-11, ZSM-12, ZSM-22, ZSM-23, ZSM-35, ZSM-38, ZSM-48, ZRP zeolite and other similar structures.Described ZSM-5 zeolite can be HZSM-5 or through element modified ZSM-5 zeolite, and element modified ZSM-5 zeolite can be one or more in phosphorus and transition metal modified ZSM-5 zeolite, for example the ZSP zeolite of phosphorus and iron modification.Described ZRP zeolite is phosphorus and rare earth modified ZRP zeolite for example.The more detailed description of relevant ZSM-5 is referring to USP3702886, and the more detailed description of relevant ZRP is referring to USP5232675, CN1211470A, CN1611299A.
Describedly contain one or more the combination that shape-selective zeolite catalysts that mean pore size is less than 0.7 nanometer can be the catalyzer that provided by prior art, can be purchased or according to existing method preparation.Described catalyzer contains zeolite, inorganic oxide and optional clay, wherein contain: 5～50 % by weight zeolites, 5～95 % by weight inorganic oxides, 0～70 % by weight clay, what described zeolite comprised that mean pore size is less than 0.7 nanometer selects shape zeolite, or also comprise optional large pore zeolite, mean pore size is less than 25～100 % by weight that shape zeolite accounts for active ingredient of selecting of 0.7 nanometer, preferred 50～100 % by weight, large pore zeolite accounts for 0～75 % by weight of active ingredient, preferably 0～50 % by weight.
Described large pore zeolite is the zeolite with the cavernous structure of at least 0.7 nano-rings opening, for example y-type zeolite, zeolite beta, zeolite L, described y-type zeolite is the mixture of one or more in rare earth Y type zeolite (REY), rare earth hydrogen y-type zeolite (REHY), ultrastable Y－type zeolite (USY), extremely steady y-type zeolite of rare earth (REUSY) for example.
Described inorganic oxide, as binding agent, is selected from silicon-dioxide (SiO
2) and/or aluminium sesquioxide (Al
2o
3).Described clay is as matrix, and carrier, can be selected from kaolin and/or halloysite.
In catalyst cracking method provided by the invention, in the second riser reactor, use contain the shape-selective zeolite catalysts that mean pore size is less than 0.7 nanometer can be identical with the first riser reactor used catalyst, also can be different.Preferably the first riser reactor and the second riser reactor use identical catalyzer.
Below in conjunction with accompanying drawing, method provided by the present invention is further described:
As shown in Figure 1, the high-temperature regenerated catalyst that flows to reactor assembly is divided into two strands, the first stock-traders' know-how regenerator inclined tube 9 enters riser reactor 1 bottom, and another stock-traders' know-how regenerator inclined tube 10 enters riser reactor 2 bottoms by regenerator inclined tube 41 after flowing to heat collector 40.Correspondingly two strands of catalyzer accelerate upwards to flow respectively under by pipeline 22 and the 23 pre-lift medium effects of injecting.Heavy feed stock after preheating (heavy hydrocarbon or be rich in the various animals and plants oils of hydrocarbon polymer) through pipeline 20 after atomizing steam from pipeline 21 mixes by a certain percentage, injecting lift pipe reactor 1, reaction oil gas is separated by oil gas carbon deposited catalyst after reaction through the fast separating device (not marking in figure) of riser tube 1 end with catalyst mixture, the gasoline fraction of simultaneously preheating or not preheating and/or C4 hydro carbons through pipeline 24 after atomizing steam from pipeline 25 mixes by a certain percentage, injecting lift pipe reactor 2, thereafter reaction oil gas and catalyst mixture upwards flow along riser tube 2, the cracking masout logistics that also can obtain with the product separation system of this device that contains certain proportion atomizing steam of introducing through pipeline 36 in path contacts, reaction, reaction oil gas and catalyst mixture be continuation reaction after the outlet sparger (not marking in figure) of riser tube 2 enters fluidized-bed reactor 4, finally enter settling vessel 5 and carry out the separated of oil gas and catalyzer.All hydrocarbon ils products, comprise the oil gas of riser tube 1 outlet and all by settling vessel top cyclone separation system (not marking figure) collection, by pipeline 30, draw reactor from the oil gas of fluidized-bed reactor 4 outflows entering subsequent product separation system 6.In product separation system 6, catalytic pyrolysis product separation is hydrocarbon gas (being drawn by pipeline 31), pyrolysis gasoline (being drawn by pipeline 32), cracking light oil (being drawn by pipeline 33), cracking masout (being drawn by pipeline 34) and cracking slurry oil (being drawn by pipeline 35).The cracked gaseous hydrocarbons that pipeline 31 is drawn can obtain polymerization-grade propylene product and be rich in the C 4 fraction of alkene after subsequent product is separated, refining, and the C 4 fraction that is wherein rich in alkene can transform production propylene by Returning reactor again.The pyrolysis gasoline that pipeline 32 is drawn partly or entirely Returning reacting system transforms again; Also can first gasoline be cut into gently, heavy naphtha section, the part or all of Returning reacting system of petroleum naphtha transforms again, preferably petroleum naphtha is returned to riser tube 2 and transforms; Any reactor of the cracking masout that pipeline 34 is drawn in can Returning reacting system transforms again, preferably partly or entirely cracking masout is introduced riser reactor 2 and/or fluidized-bed reactor 4 conversions through pipeline 36, and cracking masout entrance arrives between riser reactor outlet and/or the bottom of fluidized-bed reactor 4 at described riser reactor 2 length 1/2 places.Through the isolated carbon deposited catalyst of fast separating device of riser reactor 1 end introduce the catalyzer of fluidized-bed reactor 4 and riser tube 2 outlets mixed, react after, introduce stripper 3, stripped vapor injects through pipeline 37, with carbon deposited catalyst counter current contact, by the entrained reaction oil gas of carbon deposited catalyst, stripping is clean and cause settling vessel 5 through fluidized-bed reactor 4 as much as possible, draws settling vessel together with other oil gas through pipeline 30.Catalyzer after stripping is sent into revivifier 7 coke burning regenerations by spent agent inclined tube 8.Oxygen-containing gas is if air is through pipeline 26 injection revivifiers 7, and regenerated flue gas is drawn through pipeline 27.Catalyzer after regeneration returns to respectively riser reactor 1 and 2 through regenerator inclined tube 9 and 10 and recycles.
In above-mentioned embodiment process, by pipeline 22 and 23, to riser tube 1 and riser tube 2, introduce pre-lift medium respectively.Described pre-lift medium, for those skilled in the art know, can be selected from one or more in water vapor, C1～C4 hydro carbons or conventional catalytic cracked dry gas, preferably water steam and/or be rich in the C 4 fraction of alkene.
The following examples will be further described the present invention.
The raw material using in embodiment and comparative example comprises raw material B and raw material C, and its Raw B is a kind of atmospheric residue, and raw material C is a kind of pyrolysis gasoline that is rich in alkene, and specific nature is in Table 1.The catalyzer adopting is the catalyzer that trade names that Sinopec catalyzer asphalt in Shenli Refinery produces are MMC-2, and its specific nature is in Table 2, and what this catalyzer was less than 0.7nm containing mean pore size selects shape zeolite.
Embodiment 1
The present embodiment carries out on middle-scale device, and raw material is the pyrolysis gasoline raw material C that is rich in alkene, and catalyzer is MMC-2.In the middle-scale device of this successive reaction-regenerative operation, the internal diameter of riser tube is 16 millimeters, and length is 3200 millimeters, and leg outlet connects fluidized-bed reactor, and the internal diameter of fluidized-bed reactor is 64 millimeters, 600 millimeters of height.All raw material C charging all participates in reaction from the nozzle access to plant of riser reactor bottom.Be used for illustrating finish response situation when the mixing temperature of riser reactor bottom contact is controlled at 650 ℃, temperature of reaction and is 560 ℃.
The operating method that the present embodiment passes through with one way is carried out, and empty flows back to the pattern of refining reaction.High-temperature regenerated catalyst first carry out cold get to process by regenerated catalyst inclined tube enter riser reactor bottom, and upwards flow under the effect of water vapor pre-lift medium.Stock oil, after preheating and atomized water vapor mixing, is entered in riser tube with hot regenerated catalyst and is contacted and carry out catalytic conversion reaction by feed nozzle; Reaction mixture is along the up fluidized-bed reaction being connected with riser tube that enters by leg outlet of riser tube, oil gas after fluidized-bed reaction carries partially catalyzed agent and enters settling vessel, the fast subset arranging by settling vessel top subsequently carries out gas solid separation, and oil gas product is separated into gas and product liquid after deriving reactor by pipeline; The catalyzer that contains coke (reclaimable catalyst) after fluidized-bed reaction flows into stripper because of action of gravity, and water stripping steam stripped goes out by fluidized-bed, to enter settling vessel after the hydrocarbon product adsorbing on reclaimable catalyst and carry out gas solid separation.Reclaimable catalyst after stripping enters revivifier by reclaimable catalyst inclined tube, contacts carry out high temperature coke burning regeneration with air.Catalyzer after regeneration is processed by regenerated catalyst inclined tube and is returned in riser reactor and recycle by catalyst cooler.
The main operational condition of the present embodiment and the results are shown in table 3.
Embodiment 2
The present embodiment carries out on the middle-scale device described in example 1.All raw material C charging all participates in reaction from the nozzle access to plant of riser tube bottom.Be used for illustrating response situation when finish contact mixing temperature is controlled at 630 ℃, temperature of reaction and is 560 ℃.
The main operational condition of experiment and the results are shown in table 3.
Embodiment 3
The present embodiment carries out on the middle-scale device described in example 1.All raw material C charging all participates in reaction from the nozzle access to plant of riser tube bottom.Be used for illustrating that it is 530 ℃ of response situation during compared with low severity that finish contact mixing temperature is controlled at 580 ℃, temperature of reaction.The main operational condition of experiment and the results are shown in table 3.
Comparative example 1
Described in embodiment 1, on middle-scale device, testing.Raw material is for being rich in olefin cracking petroleum naphtha C, and catalyzer is MMC-2, and described heat-obtaining cooling process is not carried out in the agent of simulation high temperature regeneration, and the mixing temperature of finish contact is 680 ℃, and temperature of reaction is to carry out catalytic cracking reaction in 560 ℃ of situations.The main operational condition of experiment and the results are shown in table 3.
As can be seen from Table 3, catalyzer after carrying out suitable heat-obtaining cooling process again with light hydrocarbon oil contact reacts, can significantly reduce dry gas and coke yield, especially when finish initial mixing temperature is controlled at 630 ℃～650 ℃, small-numerator olefin productive rate best result is not 27.18 % by weight and 26.68 % by weight, correspondingly productivity of propylene increases respectively 2.58 and 2.08 percentage points compared with 1 of comparative example, dry gas, coke yield decline respectively 9.80,1.66 and 4.90,1.02 percentage points compared with 1 of comparative example simultaneously, and it is comparatively reasonable that product distributes.
When adopting embodiment 3 compared with low severity condition, propylene still can obtain 29.29 % by weight with total butylene one-pass yield sum, and dry gas and coking yield but can significantly reduce respectively 15.38 and 2.33 percentage points compared with comparative example 1 simultaneously.
Embodiment 4
Experiment is carried out in middle scale riser catalytic cracking unit.This middle-scale device first riser reactor internal diameter is 16 millimeters, length is 3800 millimeters, the internal diameter of the second riser reactor is 16 millimeters, length is 3200 millimeters, the second riser reactor outlet connects fluidized-bed reactor, and the internal diameter of fluidized-bed reactor is 64 millimeters, 600 millimeters of height, as shown in Figure 1, test adopts one way mode to operate to its configuration.One high-temperature regenerated catalyst enters riser reactor 1 through regenerator inclined tube 9, and upwards flows under the effect of pre-lift medium (water vapor); Stock oil B is after preheating and atomized water vapor mixing, by feed nozzle, enter in riser reactor 1, contact and carry out catalytic conversion reaction with hot regenerator, reaction oil gas and catalyst mixture carry out gas solid separation along the up oil gas exporting by riser reactor 1 of riser reactor 1 and catalyzer sharp separation equipment; After separation, oil gas is introduced product separation system 6 and is separated into gas and product liquid, and catalyzer enters fluidized-bed reactor 4 because of action of gravity.One high-temperature regenerated catalyst is cooled to 675 ℃ and is delivered to riser reactor 2 bottoms through regenerator inclined tube 41 in catalyzer heat collector 40 in addition, and upwards flow under the effect of pre-lift medium (water vapor), with the freshening light gasoline fraction from product separation system 6 (boiling range is 30～85 ℃) contact reacts of injecting from reactor 2 bottoms, then entering fluidized-bed reactor 4 reacts, reacted oil gas enters settling vessel, after isolating the catalyzer wherein carrying, introduce product separation system 6, reacted catalyzer (spent agent, comprise the catalyzer with the second riser reactor from the first riser reactor) from fluidized-bed reactor bottom enters stripper 3 strippings that are connected with fluidized-bed reactor, enter revivifier 7 and contact with air and carry out high temperature coke burning regeneration.Catalyzer after regeneration returns to two riser reactors through regenerator sloped tube and recycles.Water stripping steam stripped goes out on spent agent, after adsorbs hydrocarbons product, by fluidized-bed, to enter settling vessel and carry out gas solid separation.The main operational condition of experiment and the results are shown in table 4.
Embodiment 5
Experiment is carried out on the middle-scale device described in embodiment 4, adopts freshening mode to operate.Be not both with embodiment 4, the cracking masout cut also product separation system being obtained (boiling range is 350～500 ℃) freshening to fluidized-bed reactor bottom transforms.
After cracking masout and atomized water vapor mixing, by fluidized-bed reactor 4 bottom nozzles, enter fluidized-bed reactor 4, with catalyzer contact reacts wherein.The reacted oil gas of fluidized-bed reactor enters product separation system 6 through settling vessel, and the reacted oil gas of riser reactor 1 enters product separation system 6.
The main operational condition of experiment and the results are shown in table 4.
Comparative example 2
Described in embodiment 4, on middle-scale device, testing.This comparative example explanation: in the basic identical situation of other reaction operating mode, cracking masout does not return to the second riser tube and fluidized-bed combined reactor carries out freshening catalyzed conversion, and the high temperature regeneration agent that simultaneously enters the second riser tube and fluidized-bed combined reactor is not carried out heat-obtaining pre-treatment and reaction result direct and that light hydrocarbon oil contact catalysis transforms.The main operational condition of its experiment and the results are shown in table 4.
From table 4, the second riser tube catalyzer after outside heat removing cooling process, under the identical condition of fluidized-bed reaction temperature, the gain in yield of total liquid receipts, propylene and iso-butylene.By by cracking masout freshening to fluidized-bed reactor bottom, reduced heavy oil yield, further increased the productive rate of propylene and iso-butylene, improved the yield of high-value product.
Table 1
| Title | Raw material B | Raw material C |
| Density/(g/cm 3) | 0.8950 | 0.6696 |
| Refractive index (n d 70) | 1.4888 | / |
| Kinematic viscosity/(mm 2/s) | ||
| 80℃ | 34.92 | / |
| 100℃ | 20.09 | / |
| Condensation point/℃ | 48 | / |
| Carbon residue/m% | 6.05 | / |
| Elementary composition | ||
| (C/H)/m％ | 86.34/13.10 | 85.18/14.44 |
| (S/N)/m％ | 0.32/0.24 | 0.015/0.001 |
| Group composition | ||
| (stable hydrocarbon/aromatic hydrocarbons)/m% | 57.1/20.2 | / |
| (colloid/bituminous matter)/m% | 22.5/0.2 | / |
| (alkene)/m% | 70 | |
| Metal content/(μ g/g) | ||
| Ni/V | 18.30/0.27 | / |
| Boiling range/℃ | ||
| Initial boiling point | 278 | 32 |
| 5％ | 362 | 39 |
| 10％ | 393 | 40 |
| 30％ | 447 | 44 |
| 50％ | 503 | 48 |
| 70％ | 539(57.8) | 53 |
| 90％ | 65 | |
| 95％ | 69 |
In table 1, m represents quality
Table 2
Table 3
Table 4
Fresh feed described in table 4 refers to heavy feed stock, i.e. raw material B.
Claims (16)
1. a catalyst cracking method of producing propylene, comprising:
(1) by heavy feed stock and first strand of catalytic cracking catalyst in the first riser reactor contact reacts, tripping device by the first riser reactor end is separated with carbon deposited catalyst after reaction by oil gas, and it is separated that oil gas is introduced follow-up product separation system; What first strand of described catalytic cracking catalyst was less than 0.7nm containing mean pore size selects shape zeolite;
(2) by light hydrocarbon and temperature, be that 550 ℃～690 ℃ second strand of catalytic cracking catalysts are introduced the second riser reactor contact reacts, reacted oil gas and catalyzer introduced to the fluidized-bed reactor reaction of connecting with the second riser reactor; It is separated that the reacted oil gas of fluidized-bed reactor is introduced subsequent product separation system, the cracking masout that described product separation system separation is obtained is introduced the second riser reactor and/or fluidized-bed reactor, carbon deposited catalyst recycles after stripping, regeneration, and described light hydrocarbon comprises C4 hydrocarbon and/or the gasoline fraction that described product separation system obtains; What second strand of described catalytic cracking catalyst was less than 0.7nm containing mean pore size selects shape zeolite.
2. according to catalyst cracking method claimed in claim 1, it is characterized in that, the temperature of described second strand of catalytic cracking catalyst is 570 ℃～680 ℃.
3. according to catalyst cracking method claimed in claim 1, it is characterized in that, the weight ratio of described light hydrocarbon and heavy feed stock is 0.05～0.5: 1.
4. according to the catalyst cracking method described in claim 1～3 any one, it is characterized in that, described light hydrocarbon and second strand of catalytic cracking catalyst are 530 ℃～680 ℃ at the mixing temperature of the second riser reactor.
5. according to catalyst cracking method claimed in claim 4, it is characterized in that, described mixing temperature is 550～660 ℃.
6. according to catalyst cracking method claimed in claim 5, it is characterized in that, described mixing temperature is 630 ℃～650 ℃.
7. according to catalyst cracking method claimed in claim 1, it is characterized in that, the agent-oil ratio that described light hydrocarbon is introduced the second riser reactor reaction is 5～40.
8. according to catalyst cracking method claimed in claim 1, it is characterized in that, described light hydrocarbon is gasoline fraction and/or C4 hydrocarbon; When described light hydrocarbon comprises gasoline fraction, the operational condition that gasoline fraction reacts in the second riser reactor: agent-oil ratio is 10～30, the reaction times is 0.10～1.5 second, gasoline fraction atomized water quantity of steam accounts for 5～30 % by weight of gasoline fraction inlet amount; When described light hydrocarbon comprises C4 hydrocarbon, the operational condition that C4 hydrocarbon reacts in the second riser reactor: agent-oil ratio is 12～40, the reaction times is 0.50～2.0 second; The temperature of reaction of fluidized-bed reactor is 500～580 ℃, and weight hourly space velocity is 1～35 hour
-1.
9. according to catalyst cracking method claimed in claim 1, it is characterized in that, the temperature of reaction of the first riser reactor is 480～600 ℃, and agent-oil ratio is 5～20, and the reaction times is 0.50～10 second, and atomizing steam accounts for 2～50 % by weight of heavy feed stock inlet amount.
10. according to catalyst cracking method claimed in claim 9, it is characterized in that, the temperature of reaction of the first riser reactor is 500～560 ℃, and agent-oil ratio is 7～15, and the reaction times is 2～4 seconds, and atomized water steam accounts for 5～10 % by weight of heavy oil feedstock inlet amount.
11. according to catalyst cracking method claimed in claim 1, it is characterized in that, the cracking masout also described product separation system separation being obtained is introduced the second riser reactor and/or fluidized-bed reactor, the boiling range of described cracking masout is between 300～550 ℃, and described cracking masout is 0.01～0.35: 1 with the weight ratio that enters the heavy feed stock of the first riser reactor.
12. according to the catalyst cracking method described in claim 11, it is characterized in that, described cracking masout is introduced the second riser reactor and/or is introduced fluidized-bed reactor from fluidized-bed reactor bottom to the part of leg outlet from 1/2nd of the riser tube length of the second riser reactor.
13. in accordance with the method for claim 1, it is characterized in that, described heavy feed stock is heavy hydrocarbon and/or the various animals and plants oils that are rich in hydrocarbon polymer.
14. 1 kinds of devices for For Producing Propylene in Fcc described in claim 1, it is characterized in that, comprise riser reactor (1), riser reactor (2), fluidized-bed reactor (4), stripper (3), settling vessel (5), product separation system (6), revivifier (7) and catalyzer heat collector (40); Wherein riser reactor (2) is connected with fluidized-bed reactor (4), fluidized-bed reactor (4) is communicated with stripper (3) and settling vessel (5), riser reactor (1) is connected with settling vessel (5), and catalyzer heat collector (40) is communicated with riser reactor (2), by catalyst transport (10), is communicated with revivifier (7) by catalyst transport (41).
15. according to the device of the For Producing Propylene in Fcc described in claim 14, it is characterized in that, described riser reactor (2) length 1/2 place is provided with cracking masout entrance between riser reactor outlet and/or the bottom of fluidized-bed reactor (4).
16. according to the device for For Producing Propylene in Fcc described in claims 14 or 15, it is characterized in that, described riser reactor be selected from equal diameter riser tube, etc. linear speed riser tube and straighten same or the wherein combination of two kinds in the riser tube of footpath; That described fluidized-bed reactor is selected from is fixed fluidized bed, one or more the combination in dispersion fluidized bed, bubbling bed, turbulent bed, fast bed, conveying bed and dense bed reactor.
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| CN105349173B (en) * | 2014-08-20 | 2017-03-01 | 中国石油化工股份有限公司 | The catalytic cracking method of feed naphtha |
| CN108794292B (en) * | 2017-07-21 | 2020-03-17 | 青岛京润石化设计研究院有限公司 | Catalytic conversion method for producing more propylene |
| CN109722287B (en) * | 2017-10-30 | 2021-08-06 | 中国石油化工股份有限公司 | Catalytic conversion method for increasing propylene yield and improving light oil quality and system for method |
| CN110724561B (en) * | 2018-07-16 | 2021-03-16 | 中国石油化工股份有限公司 | Catalytic cracking method and system for producing propylene and light aromatic hydrocarbon |
| CN110724558B (en) * | 2018-07-16 | 2021-05-18 | 中国石油化工股份有限公司 | Catalytic cracking method and system for producing propylene and high-octane gasoline |
| CN110724560B (en) * | 2018-07-16 | 2021-03-16 | 中国石油化工股份有限公司 | Catalytic cracking method and system for producing propylene and light aromatic hydrocarbon |
| CN110857399B (en) * | 2018-08-24 | 2021-11-16 | 中国石油化工股份有限公司 | Method and system for processing coker gasoline and heavy raw oil by using riser |
| US11680210B2 (en) * | 2021-11-04 | 2023-06-20 | Chevron U.S.A. Inc. | Catalytic cracking of glyceride oils with deactivated phosphorus-containing ZSM-5 light olefins additives |
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